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Design and Synthesis of Fluorescent Carbon Dot Polymer and Deciphering Its Electronic Structure

Sau, Abhishek and Bera, Kallol and Pal, Uttam and Maity, Arnab and Mondal, Pritiranjan and Basak, Samrat and Mukherjee, Alivia and Satpati, Biswarup and Sen, Pintu and Basu, Samita (2018) Design and Synthesis of Fluorescent Carbon Dot Polymer and Deciphering Its Electronic Structure. Journal of Physical Chemistry C, 122 (41). pp. 23799-23807. ISSN 1932-7447. doi:10.1021/acs.jpcc.8b08322.

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Herein we report the one-pot synthesis of a fluorescent polymer-like material (pCD) by exploiting ruthenium-doped carbon dots (CDs) as building blocks. The unusual spectral profiles of pCDswith double-humped periodic excitation dependent photoluminescence (EDPL), and the regular changes in their corresponding average lifetime indicate the formation of high energy donor states and low energy aggregated states due to the overlap of molecular orbitals throughout the chemically switchable π-network of CDs on polymerization. To probe the electronic distribution of pCDs, we have investigated the occurrence of photoinduced electron transfer with a model electron acceptor, menadione using transient absorption technique, corroborated with low magnetic field, followed by identification of the transient radical ions generated through electron transfer. The experimentally obtained B_(1/2) value, a measure of the hyperfine interactions present in the system, indicates the presence of highly conjugated π-electron cloud in pCDs. The mechanism of formation of pCDs and the entire experimental findings have further been investigated through molecular modeling and computational modeling. The DFT calculations demonstrated probable electronic transitions from the surface moieties of pCDs to the tethered ligands.

Item Type:Article
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URLURL TypeDescription Information
Pal, Uttam0000-0003-2110-4610
Satpati, Biswarup0000-0003-1175-7562
Basu, Samita0000-0003-1629-2979
Additional Information:© 2018 American Chemical Society. Received: August 27, 2018; Revised: September 24, 2018; Published: September 24, 2018. We are thankful to Dr. M. K. Sarangi, C. Sengupta, R. K. Behera, A. Metya, S. Das Chakraborty, and M. Bhattacharya for their constant support and help. We are also thankful to Prof. D. Bhattachraya for his guidance in performing theoretical calculations. We acknowledge financial support from CSIR, UGC (A.S. F2-32/1998 (SA-1)), DBT-Government of India, and the BARD project: DAE at Saha Institute of Nuclear Physics. Author Contributions: A.S., K.B., and U.P. contributed equally. The authors declare no competing financial interest.
Funding AgencyGrant Number
Council of Scientific and Industrial Research (India)UNSPECIFIED
University Grants Commission (India)F2-32/1998
Department of Biotechnology (India)UNSPECIFIED
Department of Atomic Energy (India)UNSPECIFIED
Issue or Number:41
Record Number:CaltechAUTHORS:20180925-084343721
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Official Citation:Design and Synthesis of Fluorescent Carbon-Dot Polymer and Deciphering Its Electronic Structure. Abhishek Sau, Kallol Bera, Uttam Pal, Arnab Maity, Pritiranjan Mondal, Samrat Basak, Alivia Mukherjee, Biswarup Satpati, Pintu Sen, and Samita Basu. The Journal of Physical Chemistry C 2018 122 (41), 23799-23807. DOI: 10.1021/acs.jpcc.8b08322
Usage Policy:No commercial reproduction, distribution, display or performance rights in this work are provided.
ID Code:89901
Deposited By: Tony Diaz
Deposited On:25 Sep 2018 16:39
Last Modified:16 Nov 2021 00:39

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